Towards a deeper understanding of catalytic activity in supported precious metal catalysts

更深入地了解负载型贵金属催化剂的催化活性

• 批准号: EP/K007467/1
• 负责人: Andrew Beale
• 金额: $ 142.72万
• 依托单位: University College London
• 依托单位国家: 英国
• 项目类别: Fellowship
• 财政年份: 2013
• 资助国家: 英国
• 起止时间: 2013 至 无数据
• 项目状态: 已结题
• 来源: https://gtr.ukri.org/projects?ref=EP%2FK007467%2F1
• 关键词: Towards; deeper; understanding; catalytic; activity

Supported heterogeneous catalysts comprising nano-sized metals/metal oxides such as Cr, Ni, Co, Au, Pd, Pt and Ag dispersed on an oxide support (i.e. SiO2/Al2O3), play a central role in an industry estimated to be worth ca. 1500 billion $US/annum. They are the principle protagonists in the conversion of fractions from natural oil and gas to produce, via core catalytic processes (i.e. polymerisation, isomerisation, reduction and oxidation), a wide variety of chemicals for everyday use. A combination of dwindling supply and increasing demand on these feedstocks means it is vital that catalysts and catalytic processes operate as efficiently as possible. Optimal efficiency is normally achieved by rationalisation of structure with function and forms the basis for much catalysis research. However the characterisation performed is often incomplete and rarely performed under reaction conditions leading to contrasting conclusions as to what makes a catalyst active. This project will develop more robust structure-activity relationships by correlating how parameters that influence catalyst performance i.e. nanoparticle size, shape, redox functionality and metal-support interactions, affect and evolve in core catalytic processes of hydrogenation and oxidation. The project adopts a novel approach drawing on skills in catalyst preparation and in situ catalyst characterisation to prepare size-controlled monometallic nanoparticles, deposited on a flat oxide supports and to characterise them in operando using simultaneous time-resolved grazing incidence X-ray scattering (GIXRS) techniques. In particular small angle/wide angle grazing incidence scattering methods (GISAXS/GIWAXS) will be used although attempts will also be made to extract pair distribution function ((GI)PDF) from the data to enable a more complete characterisation of the catalyst. Such a thorough characterisation has never been previously employed and will be used to determine the salient characteristics of catalytic nanoparticles in both two-phase (hydrogenation) and three-phase (oxidation) catalytic systems. It is expected that these measurements will prove invaluable for understanding what makes a supported nanoparticle tick and an important basis for future catalyst optimisation and design.

包含分散在氧化物载体（即SiO2/Al 2 O3）上的纳米尺寸的金属/金属氧化物如Cr、Ni、Co、Au、Pd、Pt和Ag的负载型多相催化剂在工业中起着中心作用，估计其价值约为100亿美元。15000亿美元/年。它们是通过核心催化过程（即聚合、异构化、还原和氧化）将天然石油和天然气馏分转化为各种日常使用的化学品的主要参与者。对这些原料的供应减少和需求增加的结合意味着催化剂和催化工艺尽可能有效地运行至关重要。最佳效率通常通过结构与功能的合理化来实现，并形成了许多催化研究的基础。然而，所进行的表征通常是不完整的，并且很少在反应条件下进行，导致关于是什么使催化剂具有活性的相反结论。该项目将通过关联影响催化剂性能的参数（即纳米颗粒尺寸，形状，氧化还原功能和金属-载体相互作用）如何影响和演变加氢和氧化的核心催化过程来开发更强大的结构-活性关系。该项目采用了一种新的方法，利用催化剂制备和原位催化剂表征的技能来制备尺寸可控的monoclonal纳米颗粒，沉积在平坦的氧化物载体上，并使用同步时间分辨掠入射X射线散射（GIXRS）技术在操作中对其进行表征。特别是将使用小角/广角掠入射散射方法（GISAXS/GIWAXS），但也将尝试从数据中提取对分布函数（（GI）PDF），以实现催化剂的更完整表征。这种彻底的表征以前从未被采用过，并将用于确定两相（氢化）和三相（氧化）催化体系中催化纳米颗粒的显著特征。预计这些测量将证明是非常宝贵的了解是什么使支持的纳米粒子滴答和未来的催化剂优化和设计的重要基础。

项目成果

X-ray physico-chemical imaging during activation of cobalt-based Fischer-Tropsch synthesis catalysts.

• DOI: 10.1098/rsta.2017.0057
• 发表时间: 2018-01-13
• 期刊: Philosophical transactions. Series A, Mathematical, physical, and engineering sciences
• 作者: Beale AM;Jacques SDM;Di Michiel M;Mosselmans JFW;Price SWT;Senecal P;Vamvakeros A;Paterson J
• 通讯作者: Paterson J

Understanding the Deactivation Phenomena of Small-Pore Mo/H-SSZ-13 during Methane Dehydroaromatisation.

• DOI: 10.3390/molecules25215048
• 发表时间: 2020-10-30
• 期刊: Molecules (Basel, Switzerland)
• 作者: Agote-Arán M;Kroner AB;Wragg DS;Sławiński WA;Briceno M;Islam HU;Sazanovich IV;Rivas ME;Smith AWJ;Collier P;Lezcano-González I;Beale AM
• 通讯作者: Beale AM

Chemical imaging of the sulfur-induced deactivation of Cu/ZnO catalyst bodies

• DOI: 10.1016/j.jcat.2014.04.007
• 发表时间: 2014-05-01
• 期刊: JOURNAL OF CATALYSIS
• 影响因子: 7.3
• 作者: Beale, Andrew M.;Gibson, Emma K.;Weckhuysen, Bert M.
• 通讯作者: Weckhuysen, Bert M.

Supplementary Information from X-ray physico-chemical imaging during activation of cobalt-based Fischer-Tropsch synthesis catalysts.

钴基费托合成催化剂活化过程中 X 射线物理化学成像的补充信息。

• DOI: 10.6084/m9.figshare.5505058
• 发表时间: 2017
• 作者: Beale A

Operando HERFD-XANES/XES studies reveal differences in the activity of Fe-species in MFI and CHA structures for the standard selective catalytic reduction of NO with NH3

操作性 HERFD-XANES/XES 研究揭示了 MFI 和 CHA 结构中的铁种在标准选择性催化还原 NO 与 NH3 时的活性差异

• DOI: 10.1016/j.apcata.2018.11.026
• 发表时间: 2019-01-25
• 期刊: APPLIED CATALYSIS A-GENERAL
• 影响因子: 5.5
• 作者: Agote-Aran, Miren;Lezcano-Gonzalez, Ines;Beale, Andrew M.
• 通讯作者: Beale, Andrew M.